Radionuclides Deposition Over Antarctica M
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Journal of Environmental Radioactivity 68 (2003) 137–158 www.elsevier.com/locate/jenvrad Radionuclides deposition over Antarctica M. Pourchet a, O. Magand a,∗, M. Frezzotti b, A. Ekaykin c, J.-G. Winther d a Laboratoire de Glaciologie et Ge´ophysique de l’Environnement, CNRS, BP 96, 38402 St Martin d’He`res Cedex, France b ENEA, CLIM-OSS, P.O. Box 2400, 00100 Rome A.D., Italy c Arctic and Antarctic Research Inst., 38 Bering St., 199397 St. Petersburg, Russia d Norwegian Polar Institute, Polar Environmental Centre, Tromso, Norway Received 17 June 2002; received in revised form 11 February 2003; accepted 21 February 2003 Abstract A detailed and comprehensive map of the distribution patterns for both natural and artificial radionuclides over Antarctica has been established. This work integrates the results of several decades of international programs focusing on the analysis of natural and artificial radio- nuclides in snow and ice cores from this polar region. The mean value (37±20 Bq mϪ2)of 241Pu total deposition over 28 stations is determined from the gamma emissions of its daughter 241Am, presenting a long half-life (432.7 yrs). Detailed profiles and distributions of 241Pu in ice cores make it possible to clearly distinguish between the atmospheric thermonuclear tests of the fifties and sixties. Strong relationships are also found between radionuclide data (137Cs with respect to 241Pu and 210Pb with respect to 137Cs), make it possible to estimate the total deposition or natural fluxes of these radionuclides. Total deposition of 137Cs over Antarctica is estimated at 760 TBq, based on results from the 90–180° East sector. Given the irregular distribution of sampling sites, more ice cores and snow samples must be analyzed in other sectors of Antarctica to check the validity of this figure. 2003 Elsevier Science Ltd. All rights reserved. Keywords: Radionuclides deposition; Flux; Antarctica ∗ Corresponding author. Tel.: +33-4-76-82-42-59; fax: +33-4-76-82-42-01. E-mail address: [email protected] (O. Magand). 0265-931X/03/$ - see front matter 2003 Elsevier Science Ltd. All rights reserved. doi:10.1016/S0265-931X(03)00055-9 138 M. Pourchet et al. / J. Environ. Radioactivity 68 (2003) 137–158 1. Introduction Artificial radioisotopes resulting from atmospheric thermonuclear tests carried out between 1953 and 1980 were deposited in Antarctica after transport in the upper atmosphere and stratosphere, creating distinct radioactive reference levels in the snow. The dates of arrival and deposition in this polar region are well known and therefore provide a means to estimate Antarctic snow accumulation rates or describe air mass circulation patterns (Wilgain et al., 1965; Feely et al., 1966; Pourchet et al., 1983; Pourchet et al., 1997). The 1955 and 1965 radioactivity peaks provide two very convenient horizons for dating snow and ice layers and measuring accumu- lation. Special techniques have been developed over the last 40 yrs to detect and measure artificial and natural radionuclides present in the ice sheets (Picciotto and Wilgain, 1963; Delmas and Pourchet, 1977; Pinglot and Pourchet, 1979, 1994). In Antarctica, total beta counts remain the most frequent radioactivity measurement and are used to determine the average rate of snow accumulation (Picciotto and Wilgain, 1963; Lambert et al., 1977). Gamma profiles are also used for the determination of artificial and natural radionuclide fluxes in the region. The total deposition of artificial radionuclides (mainly 137Cs, 90Sr and 3H) and the flux of natural radionuclides (especially 210Pb) has been estimated using snow samples from many Antarctic study areas (Pourchet et al., 1997), although simul- taneous measurements of these major and complementary radionuclides in the same snow core are very rare. Snow and ice sheets on the Antarctic continent are not the only depositories of artificial and natural radionuclides deposited from the atmos- phere over the south polar region. The deposition and flux of these radionuclides have also been measured in soils, plants and lake sediments, for example on the Antarctic Peninsula (Roos et al., 1994). A detailed profile of certain radionuclides has also been obtained for the Ross Ice Shelf (Koide et al., 1979). In this work we have extended the previously available total deposition data by adding the results of a simultaneous analysis of 137Cs, 210Pb and 241Pu in the same snow cores for about 30 stations located in various parts of Antarctica and a detailed profile of these three radionuclides for Vostok and Dome Concordia stations on the Antarctic plateau area. Key results of several decades of international programs and experiments focusing on artificial radionuclide analyses of snow or ice core samples in Antarctica are used in this paper. In a previous paper (Pourchet et al., 1997), a distribution of artificial and natural radionuclides over Antarctica was proposed, based on 137Cs, 210Pb and 3H data from snow and ice-core samples. In this work, additional radioactive analysis data are used to assess and extend the previous data, increasing the significance of statistical results and validating the distribution pattern previously proposed. The evidence of a strong correlation between radionuclides may make it possible to estimate the deposition and flux of one radionuclide from available data for another one. For 210Pb, field data assess the possible double origin (unsupported and supported 210Pb) of this terrigenous radionuclide in Antarctic snow and ice-core samples, a subject already discussed by Pourchet et al. (1997). Finally, the establishment of a distri- bution pattern for artificial and natural radionuclides, which constitute isotopic tra- M. Pourchet et al. / J. Environ. Radioactivity 68 (2003) 137–158 139 cers, can help us to understand the arrival and deposition of other artificial and natural tracers via atmospheric transport. 2. Material and methods 2.1. Study area and sample description The snow and ice samples described in this paper were collected from cores or pits in different regions of the Antarctic continent, mainly in the 90–180° E sector from the Russian (Mirny to Vostok), Australian (Casey to Vostok), French (Dumont d’Urville to Dome C) and Italian (Talos Dome to Dome Concordia) transects. Ice- coring stations from other programs close to these transects were also used. Twenty-eight stations previously analyzed for 137Cs (Pourchet et al., 1997) were subject to new simultaneous 137Cs, 210Pb and 241Pu measurements. The same analyses were also performed for 24 new locations (Table 1). For Vostok and Dome Concordia stations, detailed radionuclide deposition measurements were carried out (Table 2). 2.2. Analytical methods and procedure Using a method developed by Delmas and Pourchet (1977), snow and ice core samples were melted, weighed, acidified and filtered on ion exchange paper, where all radionuclides were trapped. After drying, the filters were directly analyzed by gamma spectrometry using a low background germanium detector (Pinglot and Pourchet, 1994). Because of low activity, some samples were combined for radioac- tivity analysis (Pinglot and Pourchet, 1979, 1994). Most of the studied samples were analyzed at the LGGE laboratory in Grenoble. For high resolution gamma spec- trometry, the analyzer was protected against all interfering ambient radioactivity, in particular using an anti-Compton device. This system provides a lower detection threshold, especially for the isotopes of interest such as 137Cs (30.2 yrs), 210Pb (22.3 yrs) and 241Am (432.7 yrs), daughter of 241Pu (14.4 yrs) (Pinglot and Pourchet, 1994, 1995; Pinglot et al., 1999). Standard liquid 137Cs, 210Pb and 241Am liquids from the CEA or Amersham labora- tories (2% uncertainty at 95% of confidence level) were used to calibrate the detector. The analytical procedures were the same as those used for the snow samples. The accuracies for our measurements are about 20% for 137Cs and 210Pb and 50% for 241Am. New determinations of 137Cs for the 28 previously analyzed stations (Pourchet et al., 1997) confirm the accuracy of previous results (Fig. 1). The specific activities have been corrected for decay to the deposition time. 2.3. Measurements and determination of 241Pu and 137Cs The 241Pu and 137Cs radionuclides constitute two well-known debris products of atmospheric thermonuclear tests between 1955 and 1980. 137Cs is characteristic of both well-known reference layers in snow (1955 and 1965 peaks on beta profiles), 140 Table 1 Inventory of existing accumulation data, 137Cs and 241Pu density activities (Bq mϪ2), and 210Pb fluxes (Bq mϪ2 yrϪ1) measured and calculated in snow and ice-core samples of different zones of the Antarctic continent Stations Lat. S Long. E Elevation 10 m Snow Deposition (Bq mϪ2) 210Pb Ref. temperature accumulation M. Pourchet et al. / J. Environ. Radioactivity 68 (2003) 137 137Cs 241Pu flux deposition (°)(°)(m)(°C) (kg mϪ2 yrϪ1) (a) (b) (Bq mϪ2 yrϪ1) Ice cores M.M 77.83 167.00 20 160 164∗ n.m. n.m. 3 J9 82.37 191.33 50 Ϫ29.4 90 89 16 1.90 1 F9 84.4 189.00 50 Ϫ30.4 84 17 18 9 2.36 2 km105 67.58 93.70 1351 313 51 155 51 4.22 2 km260 68.77 94.47 2280 Ϫ33 69 44 n.m. 1.28 2 km325 69.3 95.02 2560 Ϫ37 140 95 36 5.60 2 km400 69.95 95.62 2760 Ϫ40 154 81 42 5.40 2 km200 68.25 94.08 1970 Ϫ29 271 181 99 4.48 2 VK631 72.22 96.62 3421 68 52 56 18 2.55 2 Komso 74.1 97.50 3498 Ϫ53.9 64 52 86 80 3.43 2 VK747 73.25 97.07 3270 84 40 48 29 2.26 2 VK14 78.45 106.84 3470 Ϫ55.4 23 52 34 1.20 2 VK17 78.45 106.84 3470 Ϫ55.4 19 35 38 28 2.66 2 Vostok (a) 78.45 106.84 3471 Ϫ55.4 23 58 n.m.